Publications by authors named "Christian Appel"

The functionality of materials is determined by their composition and microstructure, that is, the distribution and orientation of crystalline grains, grain boundaries and the defects within them. Until now, characterization techniques that map the distribution of grains, their orientation and the presence of defects have been limited to surface investigations, to spatial resolutions of a few hundred nanometres or to systems of thickness around 100 nm, thus requiring destructive sample preparation for measurements and preventing the study of system-representative volumes or the investigation of materials under operational conditions. Here we present X-ray linear dichroic orientation tomography (XL-DOT), a quantitative, non-invasive technique that allows for an intragranular and intergranular characterization of extended polycrystalline and non-crystalline materials in three dimensions.

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Physical exercise has been shown to induce positive reactions in bone healing but next to nothing is known about how it affects the nanostructure, in particular around implants. In this study, we established this link by using small-angle X-ray scattering tensor tomography (SASTT) to investigate nanostructural parameters in 3D such as mineral particle orientation and thickness. As a model system, rat femoral bone with a bio-resorbable implant (ultra-high purity magnesium) was used.

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Article Synopsis
  • Tomographic imaging of time-evolving samples is important but challenging, especially at the nanoscale due to limits in speed and resolution in current methods.
  • A new dynamic nanotomography technique was developed that enhances imaging efficiency using sparse dynamic imaging and 4D tomography modeling.
  • This technique significantly improves temporal resolution by 40 times and allows for detailed observations of the hydration process in polymer electrolyte fuel cell catalysts, aiding in the understanding and optimization of their performance.
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Small-angle X-ray tensor tomography and the related wide-angle X-ray tensor tomography are X-ray imaging techniques that tomographically reconstruct the anisotropic scattering density of extended samples. In previous studies, these methods have been used to image samples where the scattering density depends slowly on the direction of scattering, typically modeling the directionality, the texture, with a spherical harmonics expansion up until order ℓ = 8 or lower. This study investigates the performance of several established algorithms from small-angle X-ray tensor tomography on samples with a faster variation as a function of scattering direction and compares their expected and achieved performance.

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Heterotopic ossification (HO) in tendons can lead to increased pain and poor tendon function. Although it is believed to share some characteristics with bone, the structural and elemental compositions of HO deposits have not been fully elucidated. This study utilizes a multimodal and multiscale approach for structural and elemental characterization of HO deposits in healing rat Achilles tendons at 3, 6, 12, 16, and 20 weeks post transection.

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Polymer electrolyte fuel cells are an essential technology for future local emission-free mobility. One of the critical challenges for thriving commercialization is water management in the cells. We propose small- and wide-angle X-ray scattering as a suitable diagnostic tool to quantify the liquid saturation in the catalyst layer and determine the hydration of the ion-conducting membrane in real operating conditions.

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Intravenous (IV) iron-carbohydrate complexes are widely used nanoparticles (NPs) to treat iron deficiency anaemia, often associated with medical conditions such as chronic kidney disease, heart failure and various inflammatory conditions. Even though a plethora of physicochemical characterisation data and clinical studies are available for these products, evidence-based correlation between physicochemical properties of iron-carbohydrate complexes and clinical outcome has not fully been elucidated yet. Studies on other metal oxide NPs suggest that early interactions between NPs and blood upon IV injection are key to understanding how differences in physicochemical characteristics of iron-carbohydrate complexes cause variance in clinical outcomes.

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Calcific degeneration is the most frequent type of heart valve failure, with rising incidence due to the ageing population. The gold standard treatment to date is valve replacement. Unfortunately, calcification oftentimes re-occurs in bioprosthetic substitutes, with the governing processes remaining poorly understood.

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The complex nature of liquid water saturation of polymer electrolyte fuel cell (PEFC) catalyst layers (CLs) greatly affects the device performance. To investigate this problem, we present a method to quantify the presence of liquid water in a PEFC CL using small-angle X-ray scattering (SAXS). This method leverages the differences in electron densities between the solid catalyst matrix and the liquid water filled pores of the CL under both dry and wet conditions.

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Non-noble metal catalysts (NNMCs) hold the potential to replace the expensive Pt-based materials currently used to speed up the oxygen reduction reaction (ORR) in proton exchange membrane fuel cell (PEMFC) cathodes, but they feature poor durability that inhibits their implementation in commercial PEMFCs. This performance decay is commonly ascribed to the operative demetallation of their ORR-active sites, the electro-oxidation of the carbonaceous matrix that hosts these active centers, and/or the chemical degradation of the ionomer, active sites, and/or carbon support by radicals derived from the HO produced as an ORR by-product. However, little is known regarding the relative contributions of these mechanisms to the overall PEMFC performance loss.

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Healing large bone defects remains challenging in orthopedic surgery and is often associated with poor outcomes and complications. A major issue with bioengineered constructs is achieving a continuous interface between host bone and graft to enhance biological processes and mechanical stability. In this study, we have developed a new bioengineering strategy to produce oriented biocompatible 3D PLGA/aCaP nanocomposites with enhanced osseointegration.

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Lipid bilayers immobilized in planar geometries, such as solid-supported or "floating" bilayers, have enabled detailed studies of biological membranes with numerous experimental techniques, notably X-ray and neutron reflectometry. However, the presence of a solid support also has disadvantages as it complicates the use of spectroscopic techniques as well as surface rheological measurements that would require surface deformations. Here, in order to overcome these limitations, we investigate lipid bilayers adsorbed to inherently soft and experimentally well accessible air/water interfaces that are functionalized with Langmuir monolayers of amphiphiles.

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The acquisition speed and spatial resolution of X-ray nanotomography have continuously improved over the last decades. Coherent diffraction-based techniques breach the 10 nm resolution barrier frequently and thus pose stringent demands on sample positioning accuracy and stability. At the same time there is an increasing desire to accommodate in situ or operando measurements.

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Binary mesocrystals offer the combination of nanocrystal properties in an ordered superstructure. Here, we demonstrate the simultaneous self-assembly of platinum and iron oxide nanocubes into micrometer-sized 3D mesocrystals using the gas-phase diffusion technique. By the addition of minor amounts of a secondary particle type tailored to nearly identical size, shape and surface chemistry, we were able to promote a random incorporation of foreign particles into a self-assembling host lattice.

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Non-polar magnetic nanoparticles agglomerate upon cooling. This process is followed by in situ small angle X-ray scattering to assess structural properties of the emerging agglomerates. On the length scale of a few particle diameters, no differences are found between the agglomerates of small (d = 12 nm) and large (d = 22 nm) nanoparticles.

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Mixtures of water and PEG exhibit a well known eutectic phase diagram. While the thermodynamic properties like eutectic and liquidus temperatures as well as the eutectic concentration are intensely investigated almost nothing is known about the structural properties of water and PEG in the different regions of the phase diagram. Therefore, we report on a combined DSC, SAXS and WAXS study over the full range of polymer water compositions in order to elucidate the crystalline and semi-crystalline structure.

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Stimuli-responsive mesoporous silica films were prepared by evaporation-induced self-assembly through the physical entrapment of a functional block copolymer structuring agent, which simultaneously serves to functionalise the mesopore. These polymer-silica hybrid materials exhibit remarkable ionic permselectivity under highly filled conditions, and offer the potential for local polymer functionalisation for enhanced and tunable ionic permselectivity. This innovative and simple approach for the in situ functionalisation of mesoporous silica has the potential to improve how we approach the design of complex architectures at the nanoscale for enhanced transport, and is thus relevant for a variety of technologies based on molecular transport in nanoscale pores including separation, sensing, catalysis, and energy conversion.

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The existence of magnetic dipolar nanoparticle chains at zero field has been predicted theoretically for decades, but these structures are rarely observed experimentally. A prerequisite is a permanent magnetic moment on the particles forming the chain. Here we report on the observation of magnetic dipolar chains of spherical iron oxide nanoparticles with a diameter of 12.

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A series of poly(n-butyl acrylate) (PnBA, 5 to 32 kg mol-1) homopolymers and diblock copolymers with poly(ethylene glycol) (PEG, constant molecular weight of 0.3 kg mol-1) is synthesized for the purpose of the investigation of quasi-2D polymer films at the air-water interface. The presented compression isotherms show a transition from θ solvent behavior for PnBA homopolymers to good solvent conditions when the volume fraction of the PEG in the block copolymers is increased by decreasing the molecular weight of PnBA.

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The supramacromolecular structure of core-shell amphiphilic macromolecules (CAMs) with hyperbranched polyethyleneimine (HPEI) cores and fatty acid chain shells (HPEI-Cn) for different chain lengths was investigated both, in colloidal suspension, solid phase and at the air-water interface using Small Angle X-ray Scattering (SAXS), Wide Angle X-ray Scattering (WAXS), X-ray Reflectometry (XRR) and Langmuir isotherms. At low temperatures colloidal toluene suspensions of the HPEI-Cn polymers form, as evidenced by peaks arising in the structure factor of the system showing mean particle-to-particle distances correlated with the length of the aliphatic chains forming the shells of HPEI-Cn unimicelles. The CAM sizes as found from the SAXS experiments also display a clear dependence on shell thickness suggesting that the aliphatic chains adopt a brush-like configuration.

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